APPLIED CATALYSIS A-GENERAL
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2019
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IF 4.63
Shiqiu Zhang,Xue Yang,Kui Zheng,Ruihao Xiao,Qidong Hou,Bangjun Liu,Meiting Ju,Le Liu
It is a promising pathway to reduce the dependence on fossil fuels and obtain the bio-fuels or chemicals production from biomass derivatives. The conversion from furfural (FFR) to furfuryl alcohol (FFA) is an important industrial technology using the liquid-phase hydrogenation method with external hydrogen gas. However, the natural environment is threatened by the security of external hydrogen gas, toxicant catalyst, and the high energy consumption. Recently, in-situ hydrogenation is a novel method to converse FFR to FFA at mild reaction conditions to replace the dangerous external hydrogen gas. In this paper, we reported an efficient in-situ hydrogenation method via aqueous-phase reforming of methanol using Pt loading MgTiO 3 (perovskite-type material) at mild conditions. Pt nanoparticles were high dispersion on the nano-MgTiO 3 -450 surface, and CH 3 OH and H 2 O were reformed to produce hydrogen gas on the catalyst surface through the action of Pt nanoparticles. A part of active hydrogen could be involved in the reduction of Pt 2+ to Pt 0 , resulting in the perfect recyclability of the Pt@MT-450 catalyst. The other part of active hydrogen were participated in the hydrogenation of FFR conversion to FFA under the interaction of Pt and Mg elements. The in-situ hydrogenation of FFR to FFA using Pt@MT-450 is an effectively pathway to reduce the reaction conditions than that with external hydrogen gas.
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BIORESOURCE TECHNOLOGY
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2019
·
IF 6.669
Da Wang,Guangci Li,Chuanhui Zhang,Zhong Wang,Xuebing Li
Ni nanoparticles inlaid in lignin-derived carbon constructing the “inlaid type” Ni/C-I was reported to improve stability and adjust metal-support interaction of lignin hydrogenolysis catalyst. The Ni/C-I was further heat treated in air to prepare Ni/C-R so as to re-expose the blocked active sites by carbon species. A lot of characterization techniques were carried out to confirm the “inlaid structure” of the catalysts. The lignin depolymerization results demonstrated that the Ni/C-R had better catalytic performance than traditional “supported type” Ni/C, 23.3% aromatic monomer yield and 82.4% bio-oil yield were achieved. Moreover, the mechanism studies with lignin model compound revealed that Ni/C-R had better bond breaking ability than Ni/C, even C C bond could be cleaved. The electron effect could be responsible for that, since the electrons could transfer from Ni 0 to carbon support for Ni/C-R, which could improve the bond breaking ability.
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Chemistry-An Asian Journal
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2019
·Vol. 14
·期 13
·2266-2272
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IF 3.698
Xiaoyan Wang,Changru Huang,Xiaohao Li,Congxia Xie,Shitao Yu
Graphical PVA-encapsulated Pd nanoparticles were synthesized in water medium and applied in the hydrogenation of nitrobenzene under mild conditions. They exhibit excellent catalytic perfor-mance for the eco-friendly production of aniline. In aqueous medium without any other additives, palladium (Pd) nanoparticles with water-soluble polyvinyl alcohol (PVA) as stabilizer were synthesized for the catalytic hydrogenation of nitrobenzene. Under the optimum experimental conditions, the nitrobenzene conversion and the selectivity for aniline were 99.3 % and 100 %, respectively. Comprehensive characterization methods, including TEM, UV/Vis, confocal laser scanning microscopy (CLSM), XRD and XPS allowed a better understanding of the role of PVA aggregates and the properties of Pd nanoparticles. The nitrobenzene conversion exceeded 80 % even after 6 cycles without any treatment of the catalyst. A mechanism about the hydrogenation of nitrobenzene catalyzed by Pd/PVA system was proposed. The Pd/PVA catalyst also exhibited excellent activity and selectivity, particularly to ortho -fluoronitrobenzene and ortho -nitrotoluene. This research can provide a reference for the environmentally friendly catalysis for hydrogenation of nitrobenzene and other substituted nitrobenzene compounds.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 16
·4434-4442
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IF 9.405
Teng Li,Shengqin Liu,Bing Wang,Jingen Long,Jun Jiang,Ping Jin,Yao Fu,Haizhu Yu,Weiran Yang
Glycerol, generated in abundance as the by-product in the process of biodiesel production and saponification, has seen attempts to convert it into value-added chemicals. However, due to the low selectivity of hydrogenolysis of the secondary hydroxyl group, valuable 1,3-substituted chemicals are difficult to obtain from glycerol by chemocatalysis. In this work, glyceric acid (GA), a renewable biomass from glycerol, was quantitatively converted to 3-iodopropionic acid (3-IPA) at 373 K in 3 h by hydroiodic acid mediated hydrogenation. As the reductant in this process, HI is oxidized to I2 and then regenerated in situ by metal catalysts and H2. The reaction pathway was proposed by intermediate identification and verified by a kinetics study and computational method. The catalytic system was shown to be stable and can be reused several times without loss in activity. As a 1,3-substituted chemical, 3-IPA is not only a potential monomer to form poly-3-hydroxypropionic acid, but also a good platform molecule to produce useful chemicals, e.g. 3-hydroxypropionic acid (3-HPA) and acrylic acid (AA), due to its highly reactive nature.
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ACS Applied Materials & Interfaces
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2017
·
IF 7.504
Jin Wang,Peina Zhang,Yujiao Xiahou,Dayang Wang,Haibing Xia,Helmuth Möhwald
The present work introduces a new way to prepare Au–Pd alloy nanowire networks (NWNs) via deposition of Pd atoms onto Au nanowires in reaction media at room temperature without the aid of additional reducing agents. Thanks to their excellent colloidal stability in water as well as in ethanol, the resulting NWNs can be utilized to produce composite thin films with Nafion (perfluorinated sulfonic acid) with dimensions above dozens of square centimeters by means of solution casting on the glass substrate. Most importantly, these films can be easily transferred onto different solid substrates by lift-off technology. Moreover, the resulting Au–Pd alloy NWNs can also be easily and thoroughly loaded into macroscopic carbon fiber cloth (CFC). Both the Au–Pd alloy NWN/Nafion composite film and the Au–Pd alloy NWN-loaded CFC can be used as flexible electrodes for electrocatalysis of ethanol oxidation, with electrocatalytic performance at different distorted states superior by 2 orders of magnitude to those reported in the literature (e.g., commercial Pd/C catalysts and Pd-based nanostructured catalysts). This work opens new possibilities for the large-scale manufacturing of electrodes for fuel cells.
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Journal of Materials Chemistry A
·
2017
·Vol. 6
·期 9
·3906-3912
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IF 8.867
Jiali Sheng,Jiahui Kang,Huangqing Ye,Jinqi Xie,Bo Zhao,Xian-Zhu Fu,Yan Yu,Rong Sun,Ching-Ping Wong
Porous octahedral PdCu alloy nanocages are prepared by templating against Cu2O together with the disproportionation and displacement reactions at room temperature. Through tuning the molar ratios of the Pd/Cu precursors (PdCl42−/Cu2O), the morphology and the electrocatalysis of the octahedral PdCu nanocages can be controlled. The PdCu-5 (Pd/Cu precursor ratio of 1 : 5) nanocages exhibit superior electrocatalytic activity (1090 mA mgPd−1) towards the methanol oxidation reaction, 2.9 times higher than that of the commercial Pd/C catalyst, with remarkable durability. The combined characterization by SEM, TEM, XRD and XPS demonstrated that the excellent performance and durability of the PdCu-5 nanocages can be ascribed to their excellent hollow and porous structures as well as the electronic effect between the noble metal Pd and the cheap metal Cu. Herein, this kind of nanomaterial with novel cage-like structures is a promising catalyst for direct methanol fuel cells (DMFCs).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2017
·
IF 4.233
Sai-Sai Chen,Zhong-Zhi Yang,Ai-Jun Wang,Ke-Ming Fang,Jiu-Ju Feng
In this work, well-defined bimetallic AuPd alloyed nanocrystals (AuPd NCs) were facilely synthesized by a straightforward and controllable one-step wet-chemical strategy, using a biomolecule ( L -hydroxyproline, L -Hyp) as the green stabilizer and the structure-directing agent. Their morphology, size, composition , crystal structures and growth mechanism were investigated by a series of techniques. The synthesized architectures exhibited enlarged electrochemically active surface area (ECSA), improved catalytic activity, enhanced durability and stability towards ethylene glycol oxidation reaction (EGOR) and glycerol oxidation reaction (GOR) in alkaline electrolytes in comparison with commercial Pd black catalyst.
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Energy Technology
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2017
·Vol. 6
·期 6
·1060-1066
·
IF 2.789
Hu Li,Zhenyou Gui,Song Yang,Zhiwen Qi,Shunmugavel Saravanamurugan,Anders Riisager
Jet and diesel fuels are typically composed of C 9 -C 14 and C 12 -C 20 hydrocarbons, respectively, but the carbon-chain length of sugar-derived aldehydes and furanic compounds is no longer than C 6 . Here, a cascade catalytic process involving alkylation and hydrodeoxygenation (HDO) of 2-methylfuran (2-MF) with different aldehydes is conducted to directly produce long-chain alkanes with exclusive carbon number of C 11 -C 17 in overall yields of 50–84 %. Preliminary investigations on the alkylation of 2-MF and formalin show that the relative density of Lewis and Brønsted acidic sites of zeolitic materials remarkably affect their catalytic activity and selectivity. Sn-beta(12.5) with pronounced Lewis acidity (including the acid density and strength) exhibits higher catalytic performance in the alkylation than other zeolites, producing long-chain oxygenates in 58–92 % yields. Even in aqueous solution, the Sn-beta(12.5) catalyst can be reused for at least six reaction cycles with almost constant reactivity. More importantly, the co-addition of Hf(OTf) 4 with Pd/C greatly promotes C−O bond cleavage of the furan-ring during the HDO process under mild reaction conditions, producing long-chain alkanes in high yields of 84–94 %.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
·
IF 2.843
Lei Yang,Yuzhuo Jin,Xiangchen Fang,Zhenmin Cheng,Zhiming Zhou
Magnetic core–shell structured Pd-based catalysts (Fe3O4@M/Pd, M = SiO2, AlOOH, TiO2, Cu3(BTC)2, and ZIF-8) were prepared and applied to semihydrogenation of phenylacetylene. The catalysts were characterized by various techniques, and it was found that the predominant chemical state of Pd species on the catalyst surface was PdO2, which was stable under the reaction condition (40 °C and 0.1 MPa H2). Among all the catalysts studied, Fe3O4@ZIF-8/Pd showed the highest selectivity to styrene, which was also superior to conventional catalysts such as Pd/C, Pd/Al2O3 and Lindlar catalyst. The high selectivity of Fe3O4@ZIF-8/Pd was mainly ascribed to the electronic effect between PdO2 and ZIF-8. Further investigation revealed that the phenylacetylene hydrogenation on Fe3O4@ZIF-8/Pd was solvent-dependent with the activity increasing with the solvent polarity. Among eight solvents tested, methanol was the most effective, with high and stable selectivity to styrene (around 92%) at complete conversion of phenylacetylene (≥99.5%) during five consecutive cycles.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Aozhou Wang,Kaisheng Yao,Shuaibo Li,Qi Wang,Tianhang Han,Weiwei Lu,Haili Zhao
Furfuryl alcohol (FA) is an important chemical and has extensive applications in varied fields. To realize the highly selective hydrogenation of furfural (FF) to produce FA, the key is the preparation of the catalysts with excellent performance. Herein, a very simple wet chemical method is developed for the one-step preparation of PdAg nanosponges (NSs). Specifically, with Pd(OAc) 2 and AgNO 3 as precursors, and ethylene glycol (EG) as both solvent and reducing agent, PdAg NSs can be grown and assembled at mild temperature of 40 °C. Throughout the reaction, no any surfactants and additional reducing agents are applied. The as-prepared PdAg NSs possess 3D self-supported alloy structures, “clean” surface, abundant pores, high specific surface area and rich defects. In the FF hydrogenation reaction at 60 °C under 1.5 MPa H 2 pressure in the mixed solvent of ethanol and water (1 : 4 in volume ratio), the self-supported PdAg-1 NSs (1 : 1 in Pd/Ag molar ratio) exhibit superior catalytic performance than other PdAg NSs, pure Pd sample and commercial Pd/C (10%). With PdAg-1 NSs as catalyst in the absence of support, 100% FF can be converted and the selectivity toward FA is as high as 97.1% at 36.0 h of reaction. After 4 cycles, PdAg-1 NSs still maintain the high catalytic activity in FF hydrogenation and high selectivity toward FA, which may originate from the 3D self-supported structures, high specific surface area, “clean” surface, rich defects and electronic synergistic effect between Pd and Ag. This simple fabrication of PdAg NSs introduces new ideas for the synthesis of other nanostructured bi- and multi-metallic catalysts for highly selective FF hydrogenation to FA and other advanced applications.
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EUROPEAN POLYMER JOURNAL
·
2024
·
IF 5.8
Mengyuan Lv,Minghao Zhai,Yunlong Zang,Ziyu Zhuang,Xinying Lv,Wanan Cai,Haijun Niu,Tingting Zhou,Wen Wang
With the aim to obtain multifunctional durable electrochromic (EC) devices, we propose an effective strategy by introducing weak electron acceptor segment with suitable bandgap and oxidation potential. A series of quinoxaline-based units polyamides (PAs) (denoted as T 2 BPA-CA, T 2 BPA-OA, T 2 BPA-TP, and T 2 BPA-SA) were prepared from a novel donor–acceptor-donor (D-A-D) type diamine with weak electron acceptor quinoxaline and connected with two methoxyl-substituted donor triphenylamine, 10,13-bis[4-aminophenyl (4-methoxyphenyl) amino]-dibenzo[a,c]phenazine, and four dicarboxylic acids, which are high soluble in various organic solvents and exhibit excellent thermostability. Furthermore, the T 2 BPA-SA thin film exhibits excellent EC performance with outstanding optical contrast (50 %), high coloration efficiency (230 cm 2 C −1 ) and impressive cycle stability (optical contrast remains 80 % over 1400 cycles) in the NIR range. Meanwhile, all of these PAs are served as memristors and exhibit typical nonvolatile ternary memory, realizing an accessible threshold voltage of −0.65 V, a retention time of more than10 4 s and high current switch ratio (10 3.52 :10 2.43 :1). Overall, this work implies the great potential of these PAs in EC displays and memory storage devices.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Qingshan Zhao,Dejian Xu,Libo Wang,Shihao Cui,Qinlian Liu,Xuan Han,Zhiyuan Wang,Hui Ning,Mingbo Wu
Heteroatom doping provides an effective approach to regulating the catalytic properties of single-atom catalysts for chemical reactions. However, the economical and controllable production of efficient single-atom catalysts with tailored coordination structures presents a formidable challenge. In this study, we demonstrate a novel core-shell confinement strategy to fabricate a single-atom iron catalyst on carbon nanoshells (Fe-N/S-C) for the bifunctional selective reduction of nitroarenes and epoxidation of olefins. Through the encapsulation of polydopamine-coated nano-Fe 2 O 3 within sulfur-rich petroleum asphalt, atomically dispersed Fe-N 3 S 1 with asymmetric coordination were meticulously engineered through one-step thermal treatment, obviating the need for additional sources of iron, nitrogen, or sulfur. Under mild reaction conditions, the Fe-N/S-C catalyst achieved a complete conversion of p-nitrophenol with over 99 % selectivity and a high overall turnover frequency (TOF) of 116.9 h −1 . Meanwhile, the Fe-N/S-C catalyst could also accomplish an 80.2 % conversion in the epoxidation of styrene with a high selectivity of 93.6 %. The remarkable catalytic activities, as well as exceptional stability, notably surpass those of reported single-atom Fe-N-C and noble metal catalysts. Experimental results and theoretical calculations indicate that the negative charge induced by sulfur doping efficiently modulates the electron distribution of the active center and enhances the adsorption/desorption and activation of the reaction substrates, thereby accelerating the catalytic processes involved in selective reduction and oxidation. This work offers a promising approach to the development of cost-effective and potent catalysts for chemical transformations.
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